Optimizing the Nonlinear Optical Response of Plasmonic Metasurfaces.

Controlling the nonlinear optical response of nanoscale metamaterials opens new exciting applications such as frequency conversion or flat metal optical elements. To utilize the already well-developed fabrication methods, a systematic design methodology for obtaining high nonlinearities is required. In this paper we consider an optimization-based approach, combining a multiparameter genetic algorithm with three-dimensional finite-difference time domain (FDTD) simulations. We investigate two choices of the optimization function: one which looks for plasmonic resonance enhancements at the frequencies of the process using linear FDTD, and another one, based on nonlinear FDTD, which directly computes the predicted nonlinear response. We optimize a four-wave-mixing process with specific predefined input frequencies in an array of rectangular nanocavities milled in a thin free-standing gold film. Both approaches yield a significant enhancement of the nonlinear signal. Although the direct calculation gives rise to the maximum possible signal, the linear optimization provides the expected triply resonant configuration with almost the same enhancement, while being much easier to implement in practice.

Hybridization of graphene-gold plasmons for active control of mid-infrared radiation.

Many applications in environmental and biological sensing, standoff detection, and astronomy rely on devices that operate in the mid-infrared range, where active devices can play a critical role in advancing discovery and innovation. Nanostructured graphene has been proposed for active miniaturized mid-infrared devices via excitation of tunable surface plasmons, but typically present low efficiencies due to weak coupling with free-space radiation and plasmon damping. Here we present a strategy to enhance the light-graphene coupling efficiency, in which graphene plasmons couple with gold localized plasmons, creating novel hybridized plasmonic modes. We demonstrate a metasurface in which hybrid plasmons are excited with transmission modulation rates of 17% under moderate doping (0.35 eV) and in ambient conditions. We also evaluate the metasurface as a mid-infrared modulator, measuring switching speeds of up to 16 kHz. Finally, we propose a scheme in which we can excite strongly coupled gold-graphene gap plasmons in the thermal radiation range, with applications to nonlinear optics, slow light, and sensing.

Composite functional metasurfaces for multispectral achromatic optics.

Nanostructured metasurfaces offer unique capabilities for subwavelength control of optical waves. Based on this potential, a large number of metasurfaces have been proposed recently as alternatives to standard optical elements. In most cases, however, these elements suffer from large chromatic aberrations, thus limiting their usefulness for multiwavelength or broadband applications. Here, in order to alleviate the chromatic aberrations of individual diffractive elements, we introduce dense vertical stacking of independent metasurfaces, where each layer is made from a different material, and is optimally designed for a different spectral band. Using this approach, we demonstrate a triply red, green and blue achromatic metalens in the visible range. We further demonstrate functional beam shaping by a self-aligned integrated element for stimulated emission depletion microscopy and a lens that provides anomalous dispersive focusing. These demonstrations lead the way to the realization of ultra-thin superachromatic optical elements showing multiple functionalities-all in a single nanostructured ultra-thin element.

Subwavelength nonlinear phase control and anomalous phase matching in plasmonic metasurfaces.

Metasurfaces, and in particular those containing plasmonic-based metallic elements, constitute an attractive set of materials with a potential for replacing standard bulky optical elements. In recent years, increasing attention has been focused on their nonlinear optical properties, particularly in the context of second and third harmonic generation and beam steering by phase gratings. Here, we harness the full phase control enabled by subwavelength plasmonic elements to demonstrate a unique metasurface phase matching that is required for efficient nonlinear processes. We discuss the difference between scattering by a grating and by subwavelength phase-gradient elements. We show that for such interfaces an anomalous phase-matching condition prevails, which is the nonlinear analogue of the generalized Snell's law. The subwavelength phase control of optical nonlinearities paves the way for the design of ultrathin, flat nonlinear optical elements. We demonstrate nonlinear metasurface lenses, which act both as generators and as manipulators of the frequency-converted signal.

Nonlinear metamaterials for holography.

A hologram is an optical element storing phase and possibly amplitude information enabling the reconstruction of a three-dimensional image of an object by illumination and scattering of a coherent beam of light, and the image is generated at the same wavelength as the input laser beam. In recent years, it was shown that information can be stored in nanometric antennas giving rise to ultrathin components. Here we demonstrate nonlinear multilayer metamaterial holograms. A background free image is formed at a new frequency-the third harmonic of the illuminating beam. Using e-beam lithography of multilayer plasmonic nanoantennas, we fabricate polarization-sensitive nonlinear elements such as blazed gratings, lenses and other computer-generated holograms. These holograms are analysed and prospects for future device applications are discussed.

Rational design of metallic nanocavities for resonantly enhanced four-wave mixing.

Optimizing the shape of nanostructures and nano-antennas for specific optical properties has evolved to be a very fruitful activity. With modern fabrication tools a large variety of possibilities is available for shaping both nanoparticles and nanocavities; in particular nanocavities in thin metal films have emerged as attractive candidates for new metamaterials and strong linear and nonlinear optical systems. Here we rationally design metallic nanocavities to boost their Four-Wave Mixing response by resonating the optical plasmonic resonances with the incoming and generated beams. The linear and nonlinear optical responses as well as the propagation of the electric fields inside the cavities are derived from the solution of Maxwell's equations by using the 3D finite-differences time domain method. The observed conversion-efficiency of near-infrared to visible light equals or surpasses that of BBO of equivalent thickness. Implications to further optimization for efficient and broadband ultrathin nonlinear optical materials are discussed.